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The transition to a sustainable society is vital and requires electrification. Sodium and potassium ion-based electrolytes will likely play an important role in energy storage as these elements are very abundant. The latter cations and chloride are especially interesting since life on the planet is somehow based on biological transfers of these ions through cell membranes. K +  is the key charge carrier in plants. Here, we characterize electrochemically, electrostatically, and structurally novel electrolytes, K 3 ClO and K 2.99 Ba 0.005 ClO, and compare their performance with Na 3 ClO and Na 2.99 Ba 0.005 ClO in symmetric and asymmetric structural electrode-less cells, such as K/K 2.99 Ba 0.005 ClO in a cellulose membrane/K, Na/Na 2.99 Ba 0.005 ClO in a cellulose membrane/Na, Al/K 2.99 Ba 0.005 ClO composite/Cu, and Al/Na 2.99 Ba 0.005 ClO composite/Cu, at temperatures that range from −45 to 65 °C. An ab initio molecular dynamics structural study followed by band structure determination using density functional theory and hybrid simulations allowed us to compare the amorphous character of the structures, bandgap, and electron localization function for both K 3 ClO at 25 °C and Na 3 ClO at 37 °C, temperatures at which preliminary studies indicate that these compounds are already amorphous. As in Na + -based electrolytes, the ferroelectric character of the K + -based electrolytes is well recognizable, especially at −45 °C, where the relative real permittivity achieves 10 13  in K/K 2.99 Ba 0.005 ClO in cellulose membrane/K symmetric cells for an ionic conductivity of ∼120 mS/cm. As in Na + -based electrodes-less structural battery cells, self-charge and self-cycling phenomena are also demonstrated reinforcing the ferroelectric nature of the A 3 ClO (A = Li, Na, and K) family of electrolytes. These studies may contribute to understanding the K +  and Na +  transfer behavior in energy harvesting and storage as well as the biologic world.

Sodium and potassium ion rich ferroelectric solid electrolytes for traditional and electrode-less structural batteries